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Chlorosomes are likely the largest and most efficient naturallight-harvesting photosynthetic antenna systems. They are composed of largenumbers of bacteriochlorophylls organized into supramolecular aggregates. Weexplore the microscopic origin of the fast excitation energy transfer in thechlorosome using the recently-resolved structure and atomistic-detailsimulations. Despite the dynamical disorder effects on the electronictransitions of the bacteriochlorophylls, our simulations show that the excitondelocalizes over the entire aggregate in about 200 fs. The memory effectsassociated to the dynamical disorder assist the exciton diffusion through theaggregates and enhance the diffusion coefficients as a factor of two ascompared to the model without memory. Furthermore, exciton diffusion in thechlorosome is found to be highly anisotropic with the preferential transfertowards the baseplate, which is the next functional element in thephotosynthetic system.

Memory-assisted exciton diffusion in the chlorosome light-harvesting antenna of green sulfur bacteria